Apparatus for effecting catalytic reactions between gases under pressure and at high temperature



Jan. 5, 1932. CASALE 1,839,738

APPARATUS FOR EFFECTING CATALYTIC REACTIONS BETWEEN GASES UNDER PRESSURE AND AT HIGH TEMPERATURE Filed April 6, 1929 4 SheetsSheet l Fay. 7

Jan. 5, 1932. CASALE 1,339,738

APPARATUS FOR EFFECTING CATALYTIC REACTIONS BETWEEN GASES UNDER PRESSURE AND AT HIGH TEMPERATURE Filed April 16, 1929 4 Sheets-Sheet 2 Fig: 2

v.' f/zz/e/zfor Jan. 5, 1932. CASALE 1,839,738

APPARATUS FOR EFFECTING CATALYTIC REACTIONS BETWEEN GASES UNDER PRESSURE AND AT HIGH TEMPERATURE Filed April 16, 1929 4 Sheets-Sheet 3 [/2 1 01 for L. CASALE 1,839,738

Jam. 5, 1932.

APPARATUS FOR EFFECTING CATALYTIC REACTIONS BETWEEN GASES UNDER PRESSURE AND AT HIGH TEMPERATURE Filed April 16, 1929 4 Sheets-Sheet 4 Fly? Fl [/ZV6/2f0r Zu/y/ CczJa Z6 665 b Mavvia Charade-fa 66 74 r7zZ/rzz Patented Jan. 5, 1932 rrro STATES PATENT orFlcE IDEQEASED. LATE OF ROME, ITALY, BY mm m ADHINISTBATRIX, F ROME, ITALY was nor. EFFEGTING earn-mic nmc'rrons BETWEEN GASES impair.

PRESSURE AN D AT HIGH TEMPERATURE Application filed April 16, 1929, Serial No. 355,650, and in Italy April 85, 1928.

The industrial application of processes based upon catalytic reactions between gases under pressure and at high temperature is carried out by means of a series 0 apparatus disposed in a closed or open circuit, consisting of (a) a catalysis apparatus, (1)) a cooler in which the gases issuing from the catalytic apparatus are cooled to a suitable temperature, (c) a receiver in which are collected the products formed in the catalytic apparatus and condensed in the cooler.

There may also be inserted in the same circuit other apparatus, such as heat exchangers, in which the gas sent to the apparatus of catalysis is heated at the expense of heat from the issuing gases, gas purifiers, etc.

When the apparatus used are disposed in a closed circuit, it is necessary to use a circulating pump or another equivalent device to obtain the circulation of the reacting gases.

N ow, according to the object of the present invention, it has been found that it is possible to construct a single apparatus which will accomplish all of the operations which in the closed circuit of apparatus above re ferred to are performed by the catalysis apparatus, cooler, collector, circulating pump and heat exchanger.

Said apparatus can be constructed in va- 0 rious ways. For instance, in the annexed drawings, there is represented in Figs. 1 and 2 the vertical sections of two of the principal methods of execution.

In Fig. 1, referred to in the following description, 1 shows a steel tube able to resist the pressure of the gases contained in the tube itself; said tube is closed at the upper end by the cover 2, and at the lower end by the cover 3. Goncentrically to tube 1 is placed tube 4, at the lower end of which is fixed the cone .5, truncated by the flat surface 6 which is provided with a hole 7. Moreover, concentrically to the tube 1 are placed tubes 8, 9, 10 and 11. Tube 8, preferably lined with a thermal insulation, has the upper end free, while it is closed at the lower end by the truncated cone 12 and by the circular bottom 13, on which the lower end of the tube 11 is welded.

M5012 and 13, as well as tube 10, referred to below, will be preferably supplied with a thermal insulator. Tube 9 is closed at the lower end by disc 14 hearing in its center a hole into which is tight fitted tube 11. Tube 10 is free at its lower end. Tube 11 bears at its lower end holes 15 which allow the inside of tube 11 to communicate with the space comprised between 12 and 14.

In the upper part of the apparatus is placed block 16, the annular end 17 of which closes the free space between the upper ends of the tubes 4 and 9;block 16 closes in the upper end also the space between tubes 10 and 11 and is provided with two holes 18 and 18 through which pass the thermoelectric couples 19 and 19'. Moreover, in'block 16 there are holes which allow the space coniprised between tubes 1 and 4 to communicate with that comprised between tubes 9 and 10. In the circular space enclosed by the tube 11 is fitted the electric heating device 21. In the lower part of the apparatus 7 nal space in tube I placed below surface 5.-

In the figure is shown for this purpose a coil 24 through which flows a cold fluid which enters at 25 and issues from 26.

It is advisable that the cooler be constructed in such a manner that the gases contained in the space comprised between tubes 1 and 4 should be preventedfrom coming directly in contact with the internal surface of tube 1. Tube 1 as well as cover 2 could be supplied with cooling devices which may be independent or not from theone situated-in the space comprised between tubes 1 and 4.

Tube 27, which passes through lower cover 3, serves to admit into the apparatus the gases which are to be catalyzed. Said tube bears at its lower end a nozzle 28,which, together special piece 23, forms a true and proper ejector having a diifusion cone 22 and a suction duct 29. The gases to be catalyzed reach the nozzle compressed at a. pressure higher than the pressure existing in the apparatus and thus when entering the apparatus, they expand and part of their potential energy is transformed into kinetic energy, which is utilized by the e ector to 5 cause the circulation of gases within the apparatus itself. By means of a device which does not appear in the drawings, it is possible to displace the nozzle 28- along its axis,

thereby var ing the,position of the nozzle in respect of the difluslon cone. On the inside .of the nozzle is a regulating needle which can also be displaced along its axis by means of a special device not shown in the figures.

By working these two devices it is possible to vary within the widest possible range the velocit of the circulating gases as Well as the who between the volume of the gas circulated and the volume of the fresh gases introduced.

As shown in the illustration, the gases coming from the compressor, mixed'wlth a suitab e quantity of gases already contained in the apparatus, pass first through the space comprised between surfaces 5 and 12, and then-through the spaces comprised between 4 and 8, 8 and 9 and between surfaces 12 and 14. Thence through holes 15 they enter tube 11, in which is placed the electric heating device. The gases leave this space through holes placed in the upper end of tube 11 and then pass through the space comprised between tubes 10 and-11 which contains the catalyst.

Thence the gases pass through the space comprised between tubes 9 and 10, and then, passing through the free space 20, reach the space comprised between 1 and 4 where they are cooled to a suitable temperature by means of the devices above described. During said cooling the products formed are separated and condensed at liquid state, and are collected in s ace 31 from which they may be extracted y means of pipe 32. The gases are now suctioned through pipe 29 by the entering gases, and are again circulated through the apparatus in the manner described.

It should be observed that between the ases passing through the space comprised tween tubes Sand 9 and the gases passing through the space comprised between tubes 9 and 10 there occurs a heat-exchange in consequence of which the latter give their heat to the former. Therefore, tube 9 will by reference be provided with ribs, grooves and so on, which increase its surface.

Tube 4 will likewise be partially-or completely provided with ribs etc., since the gases which pass through the space comprised between this tube and tube 1 give a part of their heat to the gases contained in the space comprised between said tube 4 and tube 8.

Fig. 2 shows, as has been said, another manner of construction of the same apparatus 65 which differs chiefly from the preceding one on account of the two metallic blocks 33 and 34, the former placed in the up er, the latter in the lower end, each provi ed with two sets of holes, as shown in the figures which put in communication the spaces through which successively pass the gases. The position and the purpose of the two series of holes appears clearly from the figures which it is divided in two parts by its axis each showing a section so made as to show one hple of each ser1es.

Figs. 3 and 4 show two difierent ways of constructing a t e of cooler which in practice has proved hig y suitable for simultaneous- 1y cooling tube 1 and the gases passin in the space comprised between tubes 1 an 4. In the form of construction illustrated in Fig. 3, concentrically to tube 1 is placed tube 35 which, though unable to resist the pressure to which it is submitted, can, by reacting elastically to this pressure, transmit the said pressure to tube 1, which must resist to pressure, and follow this tube 1 in its deformations, so that between the contacting surfaces of tubes 1 and 35 there is always a perfect tightness. Along the external surface of tube 35, is a series of grooves through which is caused to flow the cold fluid serving to cool the gases and the tube 1 to suitable temperature. In Fig. 4 tube 35 is substituted by the two tubes 36 and 37. In both the types of construction it is advisable that the surfaces in contact with the gases be provided with ribs or grooves. By using coolers of such types any direct contact between gases and the internal surface of tube 1 is absolutely avoided.

In the examples here illustrated the gases flow six times through the upper part of the tube where the reaction and the heat exchange take place. However, apparatus can also be constructed in which the gases flow through this space a greater number of times. Likewise, the gases, instead of following the paths indicated in Figs. 1 and 2 and which are also indicated schematically in Figs. 5 and 8, can follow other paths, f. i. the paths diagrammatically represented in Figs. 6 and 7. The constructive forms corresponding to Figs. 6 and 7 are not represented in drawings, because they are easy to design on the basis of constructions represented in Figs. 1 and 2.

In the types of construction herein above described, it has been shown how the present invention is applied in the case of a synthesis tube containing a series of concentrical spaces, the innermost of which contains the electric heating device and is surrounded by an annular space containing the catalyst, the latter being in turn surrounded by other annular spaces. The present invention, however, can be applied equally to synthesis tubes having constructive forms different than the one here employed to describe the object of the present invention.

The advantages obtained using the present apparatus are:

(1) Lowering the costs of installation, owmg to the facts that the cost of an apparatus of this kind is always smaller than the total cost of the various apparatus which it substitutes, and that the space which it occupies is in practice the same as the space occupied by the synthesis tube in a plant having the same capacity of production. 0

(2) Greater simplicity of installation, resulting from the elimination of pipings which in its circuits generally employed serve to connect the varlous apparatus.

(3) Greater facility to centralize all the control and regulating devices of a synthesis unit resulting in economy in labor.

Lastly a considerable reduction in the resistance to be overcome in obtaining gas circulation, with consequent saving 1n power costs necessary to obtain said circulation.

Claims:

1. Apparatus for effecting catalytic reactions, comprising an outer, pressure resisting jacket with closed ends, a series of tubular members of different diameters mounted c0- axially in. spaced relation to each other in said jacket and suspended from the upper end thereof, the innermost of said members being open at both ends, an electric heat element secured in the upper end of said jacket and extending the entire length of said innermost member and in spaced relation thereto, the next larger member being open at the bottom only, while the three outermost members have closed bottoms and open tops, a thermo-electric couple in the s ace between two adjacent members, a gas injector axially mounted in the lower end of said jacket, a mouthpiece for the injector provided with a diffusion cone and extending between the bottom of the outermost member and the lower end of the jacket, said diffusion cone registering with an aperture in the bottom of said outermost member, the space around said nozzle forming a collecting chamber for the resulting condensate and means for draining said chamber, said mouthpiece havin gas return passages between the upper portlon of said chamber and the lower portion of the difiusion cone.

2. Apparatus for effecting catalytic reactions, comprising an outer, pressure resisting jacket with closed ends, a series of tubular members of diflerent diameters mounted coaxially in spaced relation to each other in said jacket, and suspended from the upper end thereof, the innermost of said members being open at both ends, an electric heat element secured in the upper end of said jacket and extending the entire len h of said innermost member and in space relation thereto, the next larger member being open at the bottom only, while the three outermost members have closed bottoms and open tops, a thermo-electric couple in the space between two adjacent members, a cooling coil covering substantially the entire inner surface of said jacket, a gas injector axially mounted in the lower end of said jacket, a mouthpiece for the injector provided with a diffusion cone and extending between the bottom of the outermost member and the lower end of the jacket, said diffusion cone registering with an aperture in the bottom of said outermost member, the space around said nozzle forming a collecting chamber for the resulting condensate and means for draining said chamber, said mouthpiece having gas return passages between the upper portion of said chamber and the lower portion of the diffusion cone.

3. An apparatus as described in claim 2 in which one of said tubular members is provided with heat-exchange elements.

4. An apparatus as described in claim 2 in which one of said tubular members is provided with heat-exchange elements and the tubular member adjacent thereto is provided with a thermal insulating lining.

In testimony whereof I have hereunto signed my name.

MARIA CASALE SACCHI,

Administratfiw of Luigi Oasale, deceased. 

